This comprehensive review delves into a unique intersection of hydrogels as smart molecules and their transformative applications in ophthalmology. Beginning with the foundational definition, properties, and classification of hydrogels, the review explores their synthesis and responsive capabilities. Specific applications examined encompass topical drug delivery, contact lenses, intravitreal drug delivery, ocular adhesives, vitreous substitutes, and cell‐based therapy. A methodical analysis, including an overview of relevant ocular structures and a comparative evaluation of hydrogel‐based solutions against traditional treatments, is conducted. Additionally, potential constraints, translation challenges, knowledge gaps, and research areas are identified. Our methodical approach, guided by an extensive literature review from 2017 to 2023, illuminates the unprecedented opportunities offered by hydrogels, along with pinpointing areas for further inquiry to facilitate their transition into clinical practice.